Theory Untangles the High-Resolution Infrared Spectrum of the ortho-H2-CO van der Waals Complex

Rovibrational spectroscopy of molecules boasts extremely high precision, but its usefulness relies on the assignment of spectral features to corresponding quantum mechanical transitions. In the case of ortho-H-2-CO, a weakly bound complex abundant in the interstellar medium (although not yet observed there), the rather complex spectrum has been unexplained for more than a decade. We assigned this spectrum by comparison with a purely ab initio calculation. For most lines, agreement to within 0.01 centimeter(-1) between experiment and theory was achieved. Our results show that the applicability of rovibrational spectroscopy can be extended with the assistance of high-accuracy quantum mechanical computations.